In situ h2O2 production for chemical synthesis

Ni, Fenglou 2025. In situ h2O2 production for chemical synthesis. PhD Thesis, Cardiff University. Item availability restricted.

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Abstract

The utilization of H2O2 for chemical synthesis typically provides greater selectivity compared with organic peroxides and stoichiometric oxidants, further avoiding the formation of large quantities of side products and subsequent costs for purification. However, the anthraquinone oxidation (AO) process is currently the only route to the large-scale production of H2O2, which requires large amounts of toxic solvents and huge energy input for concentration. Consequently, instead of using commercial H2O2, the production and utilization of in situ generated H2O2 from the elements (H2, O2) for the valorization of chemical feedstocks provides a more sustainable chemical synthesis route. In this thesis, two primary reactions have been investigated using heterogeneous catalysis: oxidation of methane to methanol and epoxidation of styrene to styrene oxide via in situ formation of H2O2. The direct oxidation of methane to methanol using commercial H2O2 can be operated under ambient temperatures, in comparison with the direct gas-phase methane oxidation and the indirect energy-intensive processes in industry. However, given that the cost of commercial H2O2 is typically in excess of methanol itself, it would be more promising to use in situ generated H2O2 for the conversion of methane to methanol. Therefore, in this work, the AuPd-based catalysts with different Au:Pd weight ratios were initially investigated to find out the optimal ratio for methanol production. By further utilizing the obtained optimal ratio (Au:Pd = 1:1), the effect of various supports on the catalytic activity towards methanol formation was further studied to provide insights for the development of efficient catalysts. As an important chemical feedstock, styrene oxide has been widely used in cosmetics, pharmaceuticals, etc. Given its growing demand in the global market, a more sustainable preparation process is required to replace the current procedure in the industry. However, few reports studied the epoxidation of styrene to styrene oxide using in situ generated H2O2. Thus, in this work, reaction conditions were initially investigated to verify the feasibility of the in situ styrene epoxidation reaction. Subsequently, different Pd-based bimetallic catalysts were explored to improve the formation of styrene oxide, while the reaction mechanism was further discussed to figure out the reaction pathway for styrene oxide production.

Item Type:	Thesis (PhD)
Date Type:	Completion
Status:	Unpublished
Schools:	Schools > Chemistry
Date of First Compliant Deposit:	5 August 2025
Last Modified:	05 Aug 2025 12:00
URI:	https://orca.cardiff.ac.uk/id/eprint/180269

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